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Physical review. B, Condensed matter

Hyperfine measurements of the D21 −3 H4 transition in Pr3+ : Yttrium aluminum garnet using photon echo

M. K. Kim, Ravinder Kachru

Published Aug 1, 1989• 10 citations
Publisher

Abstract

The hyperfine structure of the $^{1}\mathrm{D}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathrm{H}}_{4}$ transition of ${\mathrm{Pr}}^{3+}$: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the $^{1}\mathrm{D}_{2}$ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of ${\mathrm{Pr}}^{3+}$ impurity ions in YAG is lowered to ${C}_{2}$ from the ${D}_{2}$ symmetry of ${\mathrm{Y}}^{3+}$ ions.

DOI
10.1103/physrevb.40.2082

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Physical review. B, Condensed matter•Jun 1, 1981•22 citations
The hyperfine structure of the ^{1}\mathrm{D}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathrm{H}}_{4} transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the 1D2^{1}\mathrm{D}_{2}1D2​ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of Pr3+{\mathrm{Pr}}^{3+}Pr3+ impurity ions in YAG is lowered to C2{C}_{2}C2​ from the D2{D}_{2}D2​ symmetry of Y3+{\mathrm{Y}}^{3+}Y3+ ions.
We report a systematic study of the stimulated-photon-echo relaxation on the 3^{3}3P0{\mathit{P}}_{0}P0​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathit{H}}_{4}H4​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+:LaF3{\mathrm{LaF}}_{3}LaF3​ and the 3^{3}3P0{\mathit{P}}_{0}P0​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathit{H}}_{4}H4​ and 1^{1}1D2{\mathit{D}}_{2}D2​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathit{H}}_{4}H4​ transitions of Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (yttrium aluminum garnet). The stimulated-echo intensity is measured as a function of the delay between the first and the second pulses and the delay between the second and the third pulses. The stimulated-echo relaxation is modulated by the hyperfine interaction in the ground and the excited electronic states. We find that the modulation patterns can be quite distinct from those for two-pulse photon-echo relaxation and give complementary information about the hyperfine structures. We use the density-matrix theory of stimulated-photon-echo modulation, and the resulting simulation shows satisfactory agreement with the experimental data.
We have performed a photon echo modulation measurement of the $^{1}D_{2}\ensuremath{-}^{3}H_{4}$ levels of Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​. This time-domain method yields a precise determination of the 1D2^{1}D_{2}1D2​ excited-state hyperfine splittings and linewidths. New information on the relative orientation of the principal axes of the excited- and ground-state hyperfine Hamiltonians is presented.
When the intensity of photon echo in a two-level system is measured as a function of delay time of the two input pulses, one obtains a simple exponential decay with the characteristic phase relaxation time. When the two levels contain hyperfine structures, the interference among the hyperfine levels gives rise to modulation of the decay envelope. The Fourier transform of the modulation pattern reveals the hyperfine structure of the rare-earth ions. The hyperfine structure, and therefore the modulation pattern, are both sensitively affected by the crystal environment of the ionic site. We extend photon-echo modulation spectroscopy to three-pulse, stimulated photon-echo modulation, and we find that the stimulated echo modulation patterns are quite distinct from the two-pulse, photon-echo case and are affected by a different set of atomic and crystal interaction parameters. The modulation is measured, in several photon-echo transitions of praseodymium ions in lanthanum trifluoride and yttrium aluminum garnet crystals, as functions of delay times between first and second pulses and between first and third pulses. Comparison of the experimental results with density-matrix calculations allows us to determine hyperfine parameters that are not easily observed with two-pulse echo modulation.
Photon-echo-relaxation measurements made on the 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{3}$P0{\mathrm{P}}_{0}P0​ transition of 0.01 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (where YAG represents yttrium aluminum garnet), 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathrm{D}}_{2}D2​ transition in 0.1 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​, and 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition in 0.25 at. % Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.
The hyperfine structure and relaxation character of the terminal levels of the $^{3}P_{0}\ensuremath{-}^{3}H_{4}$ (4777 \AA{}) transition in LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ (0.03 at.%) were studied using the photon-echo technique. Using two independent nitrogen-laser pumped dye lasers we have observed modulated photon echoes for pulse separations over a \ensuremath{\sim}10-\ensuremath{\mu}sec range. In this interval our modulated photon echoes decay in a simple exponential manner by a factor of 105{10}^{5}105 and yield a homogeneous linewidth of 70 kHz [full width at half maximum (FWHM)]. Fourier transformation of the echo-modulation data yields directly the nuclear level splittings and their associated linewidths in the 3P0^{3}P_{0}3P0​ and 3H4^{3}H_{4}3H4​ states. In the 3P0(3H4)^{3}P_{0}(^{3}H_{4})3P0​(3H4​) state the nuclear splittings are 0.73 and 1.12 MHz (8.48 and 16.68 MHz). The measurements for the nuclear level splittings and associated linewidths in the 3H4^{3}H_{4}3H4​ state are in excellent agreement with those obtained from the optical-rf double-resonance experiments of Erickson. We find that the calculated echo modulation is a sensitive function of the relative orientation of the principal axes associated with the ground-and excited-state Hamiltonians. By comparing our experimental and calculated echo-modulation patterns we are able to determine their relative orientations.
Using the photon-echo-nuclear-double-resonance technique, we have measured the nuclear hyperfine splittings in the excited 1D2^{1}D_{2}1D2​ state of LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+. Our measurements are in agreement with the results obtained by Erickson from his saturated-and-enhanced-absorption study of the $^{3}H_{4}\ensuremath{-}^{1}D_{2}$ transition in LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+.